The poor photostability under ambient conditions of hybrid halide perovskites has hindered their recently explored promising nonlinear optical properties. Here, we show how Bi can partially substitute Pb homogeneously in the commonly studied MAPbI, improving both environmental stability and photostability under high laser irradiation. Bi content around 2 atom % produces thin films where the nonlinear refractive () and absorptive coefficients (β), which modify the refractive index (Δ) of the material with light fluence (), increase up to factors of 4 and 3.5, respectively, compared to undoped MAPbI. Higher doping inhibits the nonlinear parameters; however, the samples show higher fluence damage thresholds. Thus, these results provide a road map on how MAPbI can be engineered for practical cost-effective nonlinear applications by means of Bi doping, including optical limiting devices and multiple-harmonic generation into optoelectronics devices.
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